Standardization Of Radionuclides Research Articles

From Assessment of Radionuclide Contamination in Herbal Medicine Raw Material of Voronezh Region to Issues Concerning Standardization of Natural Radionuclides

From Assessment of Radionuclide Contamination in Herbal Medicine Raw Material of Voronezh Region to Issues Concerning Standardization of Natural Radionuclides

Development of multi-systems for measurement of radionuclide absolute activity

The development of a multi-systems triple-to-double coincidence ratio (TDCR) and coincidence 4pb-g methods, based on liquid scintillation to radionuclide standardization is presented in this work. The adjustments of multi-systems were made using standards of 3H and 14C and 60Co. The initial stage was performing measurements of pure beta-emitters 3H, 63Ni, and 90Sr90Y standard solutions by TDCR. The results were consistent within the standard uncertainty. Measurements will be performed with a beta-gamma 60Co in a comparison to the SIR / BIPM to assess the multi-system's performance.

Bayesian estimation of the relative deviations between activities in the radionuclide standardization

The dissemination of the activity is performed from radionuclide sources prepared in a sequence of dilutions and weighing methods. In this process, the activity of the source can be estimated statistically from the deposited mass and the activity concentration of the master solution. After preparation, the activity is obtained from absolute or relative measurement methods. However, the methods of activity determinations used may not fulfill the necessary independence of the conventional statistical approach due to the presence of possible correlations between activities that arise with the use of the same standardized sources or with the same method of quantity measurements. In this paper, Bayesian estimates for the relative deviation of activities and their uncertainty were obtained in order to evaluate the performance of the main sources’ preparation method. The estimate result (0.55 ± 0.27) % for a data set of radionuclide standardization performed between 2017 and 2018 at LNMRI, although close to zero, shows one should investigate possible effects affecting the preparation and measurement of the sources. This Bayesian estimate was validated by monte carlo simulation method.

Data analysis software package for radionuclide standardization with a digital coincidence counting system

The Nuclear Metrology Laboratory (LMN) – IPEN, São Paulo, Brazil – developed a Digital Coincidence System (DCS), based on the Coincidence Counting Methodology, in order to improve its capabilities in radionuclide primary-standardization. Digital process is implemented in two steps: data-acquisition (a set of measurements) and offline software data-analysis and calculation. The present work shows the basics of the data-acquisition unit (Software Coincidence System – SCS), describes the DCS’ data-analysis process and the initial approaches chosen for the implementation of the software package (Coincidence Analyzing Task – CAT). 152Eu standardization, performed for DCS testing, software expansion and validation, is briefly discussed.

134Cs emission probabilities determination by gamma spectrometry

The National Laboratory for Ionizing Radiation Metrology (LNMRI/IRD/CNEN) of Rio de Janeiro performed primary and secondary standardization of different radionuclides reaching satisfactory uncertainties. A solution of 134Cs radionuclide was purchased from commercial supplier to emission probabilities determination of some of its energies. 134Cs is a beta gamma emitter with 754 days of half-life. This radionuclide is used as standard in environmental, water and food control. It is also important to germanium detector calibration. The gamma emission probabilities (Pγ) were determined mainly for some energies of the 134Cs by efficiency curve method and the Pγ absolute uncertainties obtained were below 1% (k=1).

Standardization of 142Pr activity concentration

142Pr (praseodymium-142), a potential radionuclide for brachytherapy, was produced after irradiating high purity natural Pr2O3 powder in a research reactor. The irradiated powder was then dissolved in acids and diluted for measurement. Several radioactivity measurement methods were used in the standardization of 142Pr radionuclide. This work reports the results of standardization of 142Pr with CIEMAT/NIST efficiency tracing method, gamma spectrometry and a calibrated ionization chamber. The activity measured from different standardization methods are compatible with each other within the uncertainty limits. The CIEMAT/NIST efficiency tracing method gives the lowest uncertainty and is a reliable method for the standardization of this radionuclide.

TDCR and CIEMAT/NIST Liquid Scintillation Methods applied to the Radionuclide Metrology

This work presents TDCR and CIEMAT/NIST methods of liquid scintillation implemented in National Institutes of Metrology for activity standardization of radionuclides, which decay by beta emission and electron capture. The computer codes used to calculate the detection efficiency take into account: decay schemes, beta decay theory, quenching parameter evaluation, Poisson statistic model and Monte Carlo simulation for photon and particle interactions in the detection system. Measurements were performed for pure emitters 3H, 14C, 99Tc and for 68Ge/68Ga which decay by electron capture and positron emission, with uncertainties smaller than 1% (k = 1).

Performance demonstration of 4πβ(LS)-γ coincidence counting system for standardization of radionuclides with complex decay scheme

A standardization of 134Cs and 131I was carried out in order to demonstrate the performance and applicability of the 4πβ(LS)-γ coincidence counting system for standardization of radionuclides with complex decay scheme. The coincidence analyzer, capable of analyzing coincidence between beta and two gamma windows simultaneously, was developed and used for the standardization. The use of this dual coincidence analyzer has reduced the total experimental time by half. The activity concentrations obtained using the 4πβ(LS)-γ coincidence counting system, a 4πβ(PC)-γ coincidence counting system, and the CIEMAT/NIST method are in excellent agreement with each other within uncertainty limits and hence demonstrates its performance for standardization of radionuclides decaying with complex decay scheme. Hence use of this 4πβ(LS)-γ coincidence counting system can be an alternative method suitable to standardize radionuclides with complex decay scheme with acceptable precision.

Assessment of the uncertainty budget associated with 4πγ counting

The 4πγ-counting technique is recognized as a powerful primary method for the standardization of radionuclides decaying with abundant gamma emissions. Based on the use of a gamma detector in quasi 4π-geometry, a detection efficiency close to 100% and a low uncertainty can be achieved thanks to the summing effect of subsequent gamma transitions. Uncertainties have to be assigned to the realistic modelling of the source–detector geometry with respect to dimensions, density and material composition, the calculation of the total counting efficiency of the detector for the various emitted radiation, and the effect of possible flaws in the decay scheme of a radionuclide on the calculated total efficiency. Other uncertainty factors pertain to typical metrological sources of uncertainty, such as weighing, nuclear counting with pulse pile-up and system dead-time effects, impurity corrections, decay corrections, timing and frequency, etc. In order to ensure good metrological practices at NMIs, the uncertainties particular to the method are discussed.

First TDCR measurements at low energies using a miniature x-ray tube

Developed for radionuclide standardization using liquid scintillation, the Triple to Double Coincidence Ratio (TDCR) method is applied using coincidence counting obtained with a specific three-photomultiplier system. For activity determination, a statistical model of light emission is classically used to establish a relation between the detection efficiency and the experimental TDCR value. At LNE-LNHB, a stochastic approach of the TDCR modeling was developed using the Monte Carlo code Geant4. The interest of this TDCR-Geant4 model is the possibility to simulate the propagation of optical photons from their creation in the scintillation vial to the production of photoelectrons in photomultipliers.As an alternative to the use of radionuclide sources, first TDCR measurements are presented using a miniature x-ray tube closely coupled to the scintillation vial. The objective of this new set-up was to enable low-energy depositions (lower than 20keV) in liquid scintillator in order to study the influence of both time and geometrical dependence between PMTs already observed with radioactive sources. As for the statistical TDCR model, the non-linearity of light emission is implemented in the TDCR-Geant4 model using the Birks formula which depends on the kB factor and the scintillation yield. Measurements performed with the x-ray tube are extended to the assessment of these parameters and they are tested afterwards in the TDCR-Geant4 model for activity measurements of 3H.

Metrofission Project: An Overview of the ENEA Contribution

The paper describes the progress made by ENEA-INMRI in the research carried out within the framework of the Joint Research Project (JRP) ENG08 Metrofission of the European Metrology Research Programme (EMRP). This JRP aims to solve important problems related to the development of the Generation IV (GenIV) nuclear power plants in Europe as required by new demands of energy supplies that must be secure, sustainable, of high quality and also able to reduce the green house gas emissions. In the Metrofission project the ENEA-INMRI is directly involved in three Working Packages (WPs): the WP6, that aims to develop a portable Triple-to-Double-Coincidence-Ratio (TDCR) system for measuring in-situ of pure beta radionuclides; the WP7, devoted to the development of modern acquisition techniques based on Digital Coincidence Counting (DCC) with high sampling speed for radionuclide standardization; the WP8, leaded by ENEA-INMRI, which takes into account the impact of the project toward the end-users and the nuclear industry. The new prototype of the ENEA-INMRI portable TDCR counter will be presented. The preliminary results obtained in the activity measurements of 14C and 63Ni standard sources carried out by the new counter equipped with the new front-end electronics based on the CAEN Digitizer DT5720 will be discussed.

Improvements in the Monte Carlo code for simulating 4πβ(PC)–γ coincidence system measurements

A Monte Carlo simulation code known as ESQUEMA has been developed by the Nuclear Metrology Laboratory (Laboratório de Metrologia Nuclear—LMN) in the Nuclear and Energy Research Institute (Instituto de Pesquisas Energéticas e Nucleares—IPEN) to be used as a benchmark for radionuclide standardization. The early version of this code simulated only β−γ and ec−γ emitters with reasonably high electron and X-ray energies. To extend the code to include other radionuclides and enable the code to be applied to software coincidence counting systems, several improvements have been made and are presented in this work.

Application of TDCR-Geant4 modeling to standardization of 63Ni

As an alternative to the classical TDCR model applied to liquid scintillation (LS) counting, a stochastic approach based on the Geant4 toolkit is presented for the simulation of light emission inside the dedicated three-photomultiplier detection system. To this end, the Geant4 modeling includes a comprehensive description of optical properties associated with each material constituting the optical chamber. The objective is to simulate the propagation of optical photons from their creation in the LS cocktail to the production of photoelectrons in the photomultipliers. First validated for the case of radionuclide standardization based on Cerenkov emission, the scintillation process has been added to a TDCR-Geant4 modeling using the Birks expression in order to account for the light-emission nonlinearity owing to ionization quenching. The scintillation yield of the commercial Ultima Gold LS cocktail has been determined from double-coincidence detection efficiencies obtained for 60Co and 54Mn with the 4π(LS)β−γ coincidence method. In this paper, the stochastic TDCR modeling is applied for the case of the standardization of 63Ni (pure β−-emitter; Emax=66.98keV) and the activity concentration is compared with the result given by the classical model.

Application of digital sampling techniques for [formula omitted] coincidence counting

The 4 π β ( LS ) ‐ γ coincidence counting system of KRISS (Korea Research Institute of Standards and Science) has been operated in the analog signal-processing mode. We develop and implement a digital sampling method using a commercially available analog to digital converter. In the implementation, we digitize the amplified pulse trains generated from three detector channels and determine the locations and amplitudes of peaks using a peak detection algorithm. We develop offline analysis routines to process the recorded locations and amplitudes for activity determinations by means of the efficiency-extrapolation method. In the activity determinations we can make corrections for the effects of out-of-channel events and correlation between data points. We validate the digital sampling method by measuring 60Co activity and comparing the measurement results with those obtained in the analog mode. The digital method is capable of facilitating the activity standardization of radionuclides with very short half-lives.

Development of a High-Efficiency 4$\pi\beta$(LS)–$\gamma$ Coincidence System for Direct Measurements of Activity in Radioactive Decay

We developed a new 4πβ (LS)-γ coincidence counting system to be used for radionuclide standardization. The liquid scintillation detector used in this system enables the easy preparation of sources without self-absorption. A special β- β coincidence technique is implemented to suppress large thermal and electronic noises, resulting in a higher coincidence efficiency and reduced uncertainty in the measurements of low-energy beta-emitting radionuclides. The system is commissioned with the activity measurement of <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">60</sup> Co. The measured activity is derived with 90% efficiency for the β-ray detection.

Monte Carlo simulation to positron emitter standardized by means of 4πβ-γ coincidence system—Application to 22Na

The present work describes the methodology for predicting the behavior of extrapolation curves obtained in radionuclide standardization by 4pibeta-gamma coincidence measurements, applied to (22)Na, developed at the Laboratório de Metrologia Nuclear of IPEN-CNEN/SP (LMN-Nuclear Metrology Laboratory). The LMN system consists of a proportional counter (PC) in 4pi geometry coupled to a single or a pair of NaI(Tl) scintillation crystals. Two standardization techniques were used: the Sum-Peak and the Nuclear-Peak methods. The theoretical response functions of each detector have been calculated using the MCNPX Monte Carlo code. The code ESQUEMA, developed at LMN, has been used for calculating the extrapolation curve in the 4pibeta-gamma coincidence experiment. Modifications were performed in order to include response tables for positrons and coincidences with annihilation photons. From the calibration results it was possible to extract both the activity value and the positron emission probability per decay. The latter was compared with results from the literature.

Standardization of 125I by the coincidence method and practical applications

A new coincidence system, based on two thin NaI(Tl) crystals, 50×2 mm 2, with beryllium windows, 1.5 mg cm −2, positioned approximately symmetrically from the source holder (at various distances) was constructed. The electronic chains of a classical 4 πPC– γ system were utilized. A multichannel analyzer was employed for energy calibration, and an oscilloscope for visualization of the pulses. After calibration, the system was used for the standardization of an 125I solution. An energy window of 12–95 keV containing the entire spectrum (single and sum peak) was employed, and a simple demonstration of Taylor's equation [1967. X-ray–X-ray coincidence counting methods for the standardization of 125I and 197Hg. In: Standardization of Radionuclides: Proceedings of a International Atomic Energy Agency Symposium, Vienna, 1966, pp. 341–353, SM-79/65] for whole spectrum counting, was developed. The method and system were tested during the calibration of a LKB 2104 multi-gamma counter, by comparing the detection efficiency values obtained for this prepared standard solution and that utilized in the CIPM-CCRI(II) key comparison. The efficiency of the equipment was calculated as the mean of the two individual values. The result validates the method and demonstrates the accomplishment of the national traceability assurance in nuclear medicine for 125I.

Digital coincidence counting for radionuclide standardization

The 4πβ–γ coincidence method for the absolute determination of nuclear disintegration rates has for decades been successfully applied to a variety of radionuclides, via the use of suites of dedicated analogue electronic modules. The high cost of procurement and maintenance of such systems, as well as the requirement for highly experienced technicians to perform the data collection have prompted the design of more flexible data collection techniques. Recent advances in digital signal acquisition technology have facilitated the possibility of storing pulse information from multiple detector systems along with a time stamp for each recorded event, allowing various radionuclide standardization techniques (based on the concept of 4πβ–γ coincidence counting) to be implemented ‘offline’ via the use of dedicated software routines. This brief paper reviews the progress in the development of such ‘digital coincidence counting’ systems used in the field of radionuclide metrology and may be viewed as a companion article to other papers (in this issue) on primary methods for radionuclide standardization.

Radionuclide metrology using liquid scintillation counting

Liquid scintillation counting (LSC) techniques can be used for radionuclide standardization when the calculation of detection efficiency is possible. This is done using a model of the physicochemical processes involved in light emission and also of the statistics of photon emission: the free parameter model. This model can then be applied in two ways: by deducing the free parameter from the measurement of a tracer (the CIEMAT/NIST method) or by calculating this free parameter from coincidence ratio in a specific LS counter (the TDCR method). The purpose of this paper is to describe both these models and some practical issues that need to be addressed if LSC is to be effectively used in radionuclide metrology.

Quality control of liquid scintillation counters

Liquid scintillation counting (LSC) is widely used at LNHB for primary standardization of radionuclides (TDCR method), for secondary calibration and also for source stability studies or radioactive purity measurements. A total of five LSC counters are used for these purposes: two locally developed 3-photodetector counters for the implementation of the TDCR method, two Wallac 1414 counters and one Wallac 1220 Quantulus counter. The quality of the LSC measurements relies on the correct operation of these counters and their traceability to the frequency and time units.